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Initial Carbon–Carbon Bond Formation during the Early Stages of the Methanol‐to‐Olefin Process Proven by Zeolite‐Trapped Acetate and Methyl Acetate
Authors:Dr Abhishek Dutta Chowdhury  Dr Klaartje Houben  Dr Gareth T Whiting  Prof Dr Mohamed Mokhtar  Prof Dr Abdullah M Asiri  Prof Dr Shaeel A Al‐Thabaiti  Prof Dr Suliman N Basahel  Prof Dr Marc Baldus  Prof Dr Bert M Weckhuysen
Institution:1. Inorganic Chemistry and Catalysis group Debye Institute for Nanomaterials Science, Utrecht University, Utrecht, The Netherlands;2. NMR Spectroscopy, Bijvoet Center for Biomolecular Research, Utrecht University, Utrecht, The Netherlands;3. Department of Chemistry, King Abdulaziz University, Jeddah, Saudi Arabia
Abstract:Methanol‐to‐olefin (MTO) catalysis is a very active field of research because there is a wide variety of sometimes conflicting mechanistic proposals. An example is the ongoing discussion on the initial C?C bond formation from methanol during the induction period of the MTO process. By employing a combination of solid‐state NMR spectroscopy with UV/Vis diffuse reflectance spectroscopy and mass spectrometry on an active H‐SAPO‐34 catalyst, we provide spectroscopic evidence for the formation of surface acetate and methyl acetate, as well as dimethoxymethane during the MTO process. As a consequence, new insights in the formation of the first C?C bond are provided, suggesting a direct mechanism may be operative, at least in the early stages of the MTO reaction.
Keywords:methanol-to-olefin reaction  operando spectroscopy  reaction mechanisms  solid-state NMR spectroscopy  zeolites
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